Natural resilin possesses outstanding mechanical properties, such as high strain, low stiffness, and high resilience, which are difficult to be reproduced in synthetic materials. We designed high resilient elastomers (HREs) with a network structure to mimic natural resilin on the basis of two natural abundant polymers, stiff cellulose and flexible polyisoprene. With plasticization via mineral oil and mechanical cyclic tensile deformation processing, HREs show ultrahigh resilience, high strain, and reasonable tensile strength that closely mimic natural resilin. Moreover, the mechanical properties of HREs can be finely tuned by adjusting the cellulose content, providing the opportunity to synthesize high resilient elastomers that mimic different elastic proteins, such as elastin.